Deep eutectic solvent-assisted in-situ synthesis of nanosheet-packed Ni3S2 porous spheres on Ni foam for high-performance supercapacitors

Abstract Herein, self-supported Ni3S2 spherical clusters packed with well-defined nanosheets developed on Ni foam (NF) were rationally fabricated via a novel low-temperature solvothermal sulfurization approach in a choline chloride/ethylene glycol (Ethaline)-based deep eutectic solvent (DES). The DES-based sulfurization process drove an interesting time-dependent surface restructuring and phase transformation that occurred on the Ni substrate, leading to the in-situ formation of a Ni3S2 layer with controllable architecture. Pre-deposition of a Ni interlayer on the NF substrate provides more assessable electrochemical surface area and reaction sites, which favored fast crystal nucleation/growth and structural reconstruction. Benefiting from the integrated design and unique 3D interdigital architecture, the optimized Ni3S2_5/Ni/NF with a sulfurization time of 5 h exhibits a high specific capacitance (specific capacity) of 5,633 mF cm−2 (860.6 μAh cm−2) at a current density of 10 mA cm−2, and maintains 87.7% of initial specific capacitance after 1,000 charge–discharge process at a current density of 20 mA cm−2. This facile DES-driven solvothermal sulfurization strategy for the fabrication of integrated metal sulfides-based electrode materials could be promising for practical applications in high-performance electrochemical devices.